Journal of the American Chemical Society最新文献

Cathode interfacial layers (CILs) are of paramount importance in eliminating the Schottky barrier and enhancing the built-in electric field of solar cells. A profound exploration of the novel design principles for CILs and a clear elucidation of their underlying working mechanisms are undeniably crucial for developing new CIL materials and improving the performance of related devices. In this study, we meticulously designed four dipole molecules featuring different anchoring groups and intramolecular dipole moments, with the aim of conducting an in-depth investigation into the design strategy of employing dipole molecules as cathode interfacial layers. By harnessing the synergistic effect of the intramolecular dipole and the dipole formed between the anchoring group and the metal electrode, Rh-Py can significantly increase the interfacial dipole moment. This not only effectively strengthens the built-in electric field but also optimizes the ohmic contact in organic solar cells, enabling the power conversion efficiency to surpass 20% successfully. Furthermore, the strong interaction between Rh-Py and Pb²⁺ enables it to effectively passivate Pb²⁺ defects in perovskite films. When utilized as an antisolvent additive in perovskite solar cells, Rh-Py can markedly reduce nonradiative energy losses and enhance the open-circuit voltage, thereby achieving an impressive PCE of up to 25.80%. Our research findings have shed light on the design principles of fully conjugated dipolar molecules as a new type of interfacial layer material and demonstrated their versatile application potential in the fields of organic and perovskite solar cells.

The separation of acetylene (C₂H₂) and carbon dioxide (CO₂) presents significant challenges due to the similar kinetic diameters and polarities. Traditional strategies to enhance C₂H₂ binding in zeolites via weak chemisorption are hindered by limitations such as low selectivity, high-temperature desorption, and inadequate stability. Herein, by leveraging the different priority affinity for complementary electrostatic environments (C₂H₂, negative potentials; CO₂, positive potentials), we propose an innovative strategy for modulating the electrostatic potential gradient through introduction of low-charge density tetramethylammonium (TMeA⁺) cations within Y zeolite, systematically attenuating the positive electrostatic environment within the channel. This approach successfully achieves highly efficient C₂H₂/CO₂ separation in TMeA-Y-5.8 (TMeA⁺ exchanged Y zeolite with a Si/Al ratio of 5.8) while circumventing the weak chemisorption, delivering an ideal adsorbed solution theory (IAST) selectivity of 16.1 for C₂H₂/CO₂ (50/50, v/v) and a C₂H₂ adsorption capacity of 34.6 cm³/g at 10 kPa and 298 K. The dynamic C₂H₂/CO₂ separation factor of TMeA-Y-5.8 (13.1) significantly outperforms that of NaY-5.8 (3.27) and NH₄Y-5.8 (4.45) while maintaining a comparable C₂H₂ breakthrough time (C₂H₂/CO₂/Ar = 10/5/85, v/v/v, 8 mL/min, 298 K). Periodic density functional theory (DFT) calculations and differential charge density conclusively revealed a selective and significant attenuation of the interactions between CO₂ and TMeA-Y-5.8, coinciding with a diminished positive electrostatic potential within zeolite channels. Additionally, TMeA-Y-5.8 could achieve one-step purification of C₂H₂ from a ternary mixture of C₂H₂/C₂H₄/CO₂. The exceptional regeneration capability (333 K), outstanding moisture resistance, and stable recyclability of TMeA-Y-5.8 collectively demonstrate the effectiveness and practical applicability of this electrostatic potential gradient modulation strategy.